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镍基催化剂上积碳是甲烷干气重整反应急需解决的关键问题。实验采用TPSR、TPD、XPS和脉冲反应等方法系统研究了镍基催化剂表面积碳的形态和特点。热力学研究表明,在573 K到1273 K的温度范围内,催化剂的表面积碳是不可避免的。TPSR、XPS和TPD研究表明,甲烷在催化剂表面裂解将形成至少三种碳物种:Cα、Cβ和Cγ。这三种碳物种具有不同的表面迁移能力、热稳定性和反应活性。其中,Cα物种在甲烷干气重整反应中是一种非常活泼和重要的中间体;Cγ物种则可能是表面积碳的前驱物:部分脱氢的Cβ物种能够与H2或CO2反应生成CH4或CO。
Nickel-based catalyst for carbon deposition is the critical problem to be solved urgently for methane dry gas reforming reaction. In the experiment, the morphology and characteristics of surface area carbon of Ni-based catalysts were systematically investigated by TPSR, TPD, XPS and pulse reaction. Thermodynamic studies show that the surface carbon deposition of the catalyst is unavoidable in the temperature range of 573 K to 1273 K. TPSR, XPS and TPD studies have shown that methane cracking on the catalyst surface will form at least three carbon species: Cα, Cβ and Cγ. These three carbon species have different surface mobility, thermal stability and reactivity. Among them, Cα species is a very active and important intermediate in dry gas reforming of methane; Cγ species may be a precursor of surface carbon deposition: partially dehydrogenated Cβ species can react with H2 or CO2 to form CH4 or CO .